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Tailoring Gold Nanoparticle Characteristics and the Impact on Aqueous-Phase Oxidation of Glycerol

DOI: 10.1021/acscatal.5b00754 DOI Help

Authors: Scott Rogers (Rutherford Appleton Laboratory; University College London (UCL)) , C. Richard A. Catlow (Rutherford Appleton Laboratory; University College London (UCL)) , Carine E. Chan-thaw (Universita degli Studi di Milano) , Diego Gianolio (Diamond Light Source) , Emma Gibson (University College London) , Anna Gould (Rutherford Appleton Laboratory; University College London (UCL)) , Nan Jian (University of Birmingham) , Andrew J. Logsdail (University College London) , Richard E. Palmer (University of Birmingham) , Laura Prati (Universita degli Studi di Milano) , Nikolaos Dimitratos (The UK Catalysis Hub, Research Complex at Harwell, U.K.) , Alberto Villa (Universita degli Studi di Milano) , Peter Wells (Rutherford Appleton Laboratory; University College London (UCL))
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Acs Catalysis , VOL 5 (7) , PAGES 4377 - 4384

State: Published (Approved)
Published: July 2015
Diamond Proposal Number(s): 8071

Open Access Open Access

Abstract: Poly(vinyl alcohol) (PVA)-stabilized Au nanoparticles (NPs) were synthesized by colloidal methods in which temperature variations (−75 to 75 °C) and mixed H2O/EtOH solvent ratios (0, 50, and 100 vol/vol) were used. The resulting Au NPs were immobilized on TiO2 (P25), and their catalytic performance was investigated for the liquid phase oxidation of glycerol. For each unique solvent system, there was a systematic increase in the average Au particle diameter as the temperature of the colloidal preparation increased. Generation of the Au NPs in H2O at 1 °C resulted in a high observed activity compared with current Au/TiO2 catalysts (turnover frequency = 915 h–1). Interestingly, Au catalysts with similar average particle sizes but prepared under different conditions had contrasting catalytic performance. For the most active catalyst, aberration-corrected high angle annular dark field scanning transmission electron microscopy analysis identified the presence of isolated Au clusters (from 1 to 5 atoms) for the first time using a modified colloidal method, which was supported by experimental and computational CO adsorption studies. It is proposed that the variations in the populations of these species, in combination with other solvent/PVA effects, is responsible for the contrasting catalytic properties.

Journal Keywords: Gold Nanoparticles; Colloids; Xafs; Glycerol Oxidation; Heterogeneous Catalysis; Aberration-Corrected Tem

Subject Areas: Biology and Bio-materials


Instruments: B18-Core EXAFS